EP0649877A2 - Compositions autolubrifiantes - Google Patents

Compositions autolubrifiantes Download PDF

Info

Publication number
EP0649877A2
EP0649877A2 EP94116179A EP94116179A EP0649877A2 EP 0649877 A2 EP0649877 A2 EP 0649877A2 EP 94116179 A EP94116179 A EP 94116179A EP 94116179 A EP94116179 A EP 94116179A EP 0649877 A2 EP0649877 A2 EP 0649877A2
Authority
EP
European Patent Office
Prior art keywords
phosphoric acid
mixtures according
acid ester
weight
silicone rubber
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP94116179A
Other languages
German (de)
English (en)
Other versions
EP0649877B1 (fr
EP0649877A3 (fr
Inventor
Dieter Dr. Wrobel
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Momentive Performance Materials GmbH
Original Assignee
Bayer AG
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Bayer AG filed Critical Bayer AG
Publication of EP0649877A2 publication Critical patent/EP0649877A2/fr
Publication of EP0649877A3 publication Critical patent/EP0649877A3/fr
Application granted granted Critical
Publication of EP0649877B1 publication Critical patent/EP0649877B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00Use of organic ingredients
    • C08K5/49Phosphorus-containing compounds
    • C08K5/51Phosphorus bound to oxygen
    • C08K5/52Phosphorus bound to oxygen only
    • C08K5/521Esters of phosphoric acids, e.g. of H3PO4
    • C08K5/523Esters of phosphoric acids, e.g. of H3PO4 with hydroxyaryl compounds
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L83/00Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
    • C08L83/04Polysiloxanes
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G77/00Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
    • C08G77/04Polysiloxanes
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G77/00Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
    • C08G77/04Polysiloxanes
    • C08G77/20Polysiloxanes containing silicon bound to unsaturated aliphatic groups
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G77/00Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
    • C08G77/04Polysiloxanes
    • C08G77/22Polysiloxanes containing silicon bound to organic groups containing atoms other than carbon, hydrogen and oxygen
    • C08G77/24Polysiloxanes containing silicon bound to organic groups containing atoms other than carbon, hydrogen and oxygen halogen-containing groups

Definitions

  • the present invention relates to mixtures with self-lubricating properties in the cured state, comprising at least one crosslinkable silicone rubber a), at least one aryl phosphoric acid ester b) and at least one further additive c), a process for their preparation and moldings based on these mixtures.
  • Self-lubricating silicones are known per se: According to EP 369 255 (Description of the Prior Art), for example, copolymers with diethylsiloxy and diphenylsiloxy units with a significant proportion of diphenylsiloxy groups are only suitable for this purpose to a limited extent, since the exudation behavior is often unpredictable and the lubricating effect is often absent.
  • Short-chain OH-terminated diorganosiloxanes with trifluoropropyl groups in peroxidically crosslinked systems should not have this disadvantage (EP 369 255).
  • OH-terminated oils are not suitable for addition-crosslinking silicone rubbers which contain hydrogen siloxanes as crosslinkers.
  • the OH-terminated polymers also react with the hydrogen siloxanes to form an SiOSi bond: ⁇ Si ⁇ OH + H ⁇ Si ⁇ ⁇ ⁇ Si-O-Si ⁇ + H2 They are integrated into the network and can no longer migrate to the surface and form a lubricating film there.
  • both types of oil have other disadvantages. They consist of polymers of different chain lengths, which inevitably cause fluctuating molecular weight distributions. Accordingly, the sweating behavior fluctuates more or less strongly.
  • Another disadvantage for technical use is the high prices of these special silicone oils.
  • the object of the present invention is therefore to provide mixtures which, in the hardened state, have self-lubricating properties.
  • the present invention relates to mixtures with self-lubricating properties in the cured state which contain at least one silicone rubber a), at least one aryl phosphoric acid ester b) and at least one further additive c) in which the aryl phosphoric acid ester used is incompatible with silicone.
  • Silicone rubbers a) for the purposes of the invention are substances known per se, as described, for example, in W. Noll "Chemistry and Technology of Silicones", 1968, page 246.
  • Component a) preferably corresponds to a silicone rubber of the following formula (II) wherein R and R 'are alkyl radicals with 1 to 8 carbon atoms, aryl radicals, vinyl radicals and fluoroalkyl radicals with 3 to 8 carbon atoms, so that the polymer contains 0.0002 to 3 wt .-% vinyl groups, and x is varied so that the viscosity of the Polymers ranges from 0.1 to 30,000 Pa.s,
  • the silicone rubber may optionally contain fillers and water repellents.
  • Hydrophobing agents in the sense of the invention are preferably silanol-containing silicone compounds with a viscosity of 0.01 to 1 Pa.s and / or hexaalkyldisilazanes, the organic groups being selected from alkyl radicals with 1 to 8 carbon atoms, vinyl radicals, aryl radicals and fluoroalkyl radicals with 3 to 8 carbon atoms that the silicone compounds have a silanol content (content of S: OH groups) of 2 to 10 wt .-%.
  • Suitable fillers for the process according to the invention are e.g. pyrogenic or precipitated, finely divided silicas with a BET surface area of 50 to 500 m2 / g.
  • Such fillers can be surface modified, e.g. with organosilicon compounds. The modification can also be carried out during incorporation into the polymer by adding e.g. Hexamethyldisilazane and / or 1,3-divinyl-1,1,3,3-tetramethyldisilazane can be achieved with the addition of water.
  • Substances such as diatomaceous earth, finely divided quartz powder, amorphous silicas or carbon blacks can also be used as fillers.
  • the silicone rubber a) can be both an addition-crosslinking silicone rubber with hydrogen siloxane as crosslinker a ') and a peroxidically crosslinkable silicone rubber a' ').
  • the mixture preferably contains the hydrogen siloxanes described below as crosslinkers where R 'are alkyl radicals with 1 to 8 carbon atoms or aryl and fluoroalkyl radicals with 3 to 8 C atoms, m ⁇ 3 and n + m varies so that the polymer has a viscosity of 0.005 to 1 Pa.s, and additionally one Rhodium or platinum catalyst and possibly inhibitors and other auxiliaries.
  • the platinum catalysts are the catalysts usually used for the addition-crosslinking systems, in particular Pt (0) complexes with vinylsiloxanes as ligands.
  • Suitable inhibitors are acetylenic alcohols such as 2-methylbutin (3) -ol- (2), ethinylcyclohexanol, tetramethyltetravinylcyclotetrasiloxane or tetramethyldivinyldisiloxane.
  • Peroxidically crosslinking compositions preferably contain alkyl or aryl peroxides, such as, for example, the hydrogen siloxanes and the catalyst.
  • alkyl or aryl peroxides such as, for example, the hydrogen siloxanes and the catalyst.
  • the aryl phosphoric acid esters used according to the invention are generally commercially available products.
  • the aryl phosphoric acid ester b) preferably has the general formula (I) in the R1 and R2 phenyl, alkylphenyl, ⁇ -methylbenzylphenyl, alkyl radicals and R3 is phenyl, alkylphenyl, ⁇ -methylbenzylphenyl.
  • alkyl radicals linear C1-C8 radicals are preferably used.
  • Additives c) in the sense of the invention are preferably unreactive, non-inhibiting, silicone-incompatible oils, such as, for example, trifluoropropylmethyl silicone oil, paraffin oil and plasticizer oils, such as adipic acid esters and polyesters.
  • silicone-incompatible oils such as, for example, trifluoropropylmethyl silicone oil, paraffin oil and plasticizer oils, such as adipic acid esters and polyesters.
  • the level of addition of aryl phosphoric acid ester b) depends essentially on the hardness of the vulcanizate and the desired amount of exudation as well as the degree of incompatibility of the aryl phosphoric acid ester.
  • the amount of the aryl phosphoric acid ester is preferably 0.5 to 10% by weight, particularly preferably 3 to 10% by weight, the amount of the additives is preferably 0.5 to 5% by weight, based on the total mixture.
  • the present invention also relates to a process for the preparation of these silicone compositions, according to which components a) to c) are stirred together.
  • the present invention also relates to moldings with self-lubricating properties, which can be obtained by introducing components a) and b) and optionally c) into a mold and subsequent vulcanization at elevated pressure and a temperature of 50 to 250 ° C.
  • this silicone base composition are mixed with 1.53 g of a trimethylsilyl end-blocked polyorganosiloxane crosslinking agent with an average of 5 methylhydrogensiloxane units and 3 dimethylsiloxane units per molecule, 0.15 g of a platinum catalyst in the form of a complex of chloroplatinic acid with symmetrical divinyltetramethyldisiloxane and containing about 0.65% platinum and about 0.65% platinum and , 02 g of 3,5-dimethyl-1-hexin-3-ol as an inhibitor and 1.5 parts of diphenyl cresyl phosphate are mixed and cured under pressure for 10 minutes at 175 ° C. in a 2 mm thick mold. After storage for 1 day at room temperature, the surface
  • a dimethylpolysiloxane (0.02% vinylsiloxy units) with a chain length of 6000 units and a viscosity of 20.106 mPas, ends limited by trimethylsiloxy groups, are mixed with 53.5 parts by weight of a silica with a BET surface area of 200 m2 / g in a kneader at 150 ° C.
  • a siloxanol with 18% SiOH groups and 4.2 parts of a siloxanol, which additionally contains 5% vinylmethylsiloxy units, and 0.55 parts of hexamethyldisilazane are added.
  • Example 11 but additionally with 1.0 part of diphenyl cresyl phosphate. After storage for 1 day at room temperature, the surface is covered with a thin film of oil.
  • Example 11 As in Example 11, but with 0.5 part of copolymer oil (from Example 11) and additionally 1.1 parts of diphenyl cresyl phosphate. After storage for 1 day at room temperature, the surface is covered with a thin film of oil.
  • Example 11 As in Example 11, but with 1.9 parts of copolymer oil (from Example 11). After storage for 1 day at room temperature, the surface shows fluctuating properties from dry to slightly lubricating.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Lubricants (AREA)
  • Processes Of Treating Macromolecular Substances (AREA)
EP94116179A 1993-10-26 1994-10-13 Compositions autolubrifiantes Expired - Lifetime EP0649877B1 (fr)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
DE4336472 1993-10-26
DE4336472 1993-10-26
DE4408660 1994-03-15
DE4408660A DE4408660A1 (de) 1993-10-26 1994-03-15 Mischungen mit selbstschmierenden Eigenschaften

Publications (3)

Publication Number Publication Date
EP0649877A2 true EP0649877A2 (fr) 1995-04-26
EP0649877A3 EP0649877A3 (fr) 1996-05-01
EP0649877B1 EP0649877B1 (fr) 2001-03-28

Family

ID=25930721

Family Applications (1)

Application Number Title Priority Date Filing Date
EP94116179A Expired - Lifetime EP0649877B1 (fr) 1993-10-26 1994-10-13 Compositions autolubrifiantes

Country Status (7)

Country Link
US (1) US5583170A (fr)
EP (1) EP0649877B1 (fr)
JP (1) JPH07179759A (fr)
AT (1) ATE200099T1 (fr)
CA (1) CA2134042A1 (fr)
DE (2) DE4408660A1 (fr)
ES (1) ES2156887T3 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2001090230A1 (fr) * 2000-05-26 2001-11-29 Nkt Research A/S Polymeres autolubrifiants
WO2005054370A3 (fr) * 2003-12-03 2006-01-05 Clariant Gmbh Agents antimousse
EP1958988A1 (fr) 2007-02-15 2008-08-20 Wacker Chemie AG Compositions de silicone réticulables par addition présentant und faible coefficient de friction

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6871838B2 (en) * 2003-04-03 2005-03-29 B. Braun Medical Inc. Injection port valve
US7205050B2 (en) * 2003-06-09 2007-04-17 Permatex, Inc. Low shear adhesion RTV silicone
US7527703B2 (en) * 2004-09-09 2009-05-05 Jeffrey Swain Submerged masonry surface treating method
JP7359861B2 (ja) 2019-03-29 2023-10-11 ダウ シリコーンズ コーポレーション シリコーンエラストマー組成物及びエラストマー材料

Family Cites Families (13)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3288743A (en) * 1966-11-29 Plasticized polyorganosilsesquioxane compositions
US2618600A (en) * 1948-07-15 1952-11-18 Douglas Aircraft Co Inc Silicone oil lubricating composition
US2684336A (en) * 1950-06-02 1954-07-20 Douglas Aircraft Co Inc Silicone lubricant containing trialkyl phosphate
DE2535334B2 (de) * 1975-08-07 1978-09-28 Bayer Ag, 5090 Leverkusen Verfahren zur homogenen Verteilung hochdisperser aktiver Füllstoffe in Poly organosiloxanen
DE2708447A1 (de) * 1976-03-06 1977-09-08 Ciba Geigy Ag Flammhemmende polymerzusammensetzungen
DE2653499C3 (de) * 1976-11-25 1980-05-08 Wacker-Chemie Gmbh, 8000 Muenchen Unter Ausschluß von Wasser lagerfähige bei Zutritt desselben bei Raumtemperatur zu Elastomeren vernetzende Organopolysiloxanformmassen
JPS57141476A (en) * 1981-02-25 1982-09-01 Haraden Koji Kk Refractory airtight sealing material
US4497692A (en) * 1983-06-13 1985-02-05 International Business Machines Corporation Laser-enhanced jet-plating and jet-etching: high-speed maskless patterning method
JPS6241263A (ja) * 1985-08-16 1987-02-23 Shin Etsu Chem Co Ltd 動的疲労耐久性シリコ−ンゴム組成物
DE59000647D1 (de) * 1989-07-20 1993-02-04 Duering Ag Faltbare kunststoff-flasche.
DE4016417A1 (de) * 1990-05-22 1991-11-28 Bayer Ag Flammwidrige polycarbonate
DE69223550T2 (de) * 1991-05-28 1998-04-16 Denki Kagaku Kogyo Kk Flammhemmende Harzzusammensetzung
US5412014A (en) * 1992-06-29 1995-05-02 Dow Corning Corporation Fire retardant resin compositions

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2001090230A1 (fr) * 2000-05-26 2001-11-29 Nkt Research A/S Polymeres autolubrifiants
WO2005054370A3 (fr) * 2003-12-03 2006-01-05 Clariant Gmbh Agents antimousse
EP1958988A1 (fr) 2007-02-15 2008-08-20 Wacker Chemie AG Compositions de silicone réticulables par addition présentant und faible coefficient de friction
DE102007007569A1 (de) 2007-02-15 2008-08-21 Wacker Chemie Ag Additionsvernetzbare Siliconmassen mit geringen Reibungskoeffizienten
US7803868B2 (en) 2007-02-15 2010-09-28 Wacker Chemie Ag Addition-crosslinkable silicone compositions with low coefficients of friction

Also Published As

Publication number Publication date
ES2156887T3 (es) 2001-08-01
ATE200099T1 (de) 2001-04-15
EP0649877B1 (fr) 2001-03-28
EP0649877A3 (fr) 1996-05-01
JPH07179759A (ja) 1995-07-18
DE59409702D1 (de) 2001-05-03
US5583170A (en) 1996-12-10
DE4408660A1 (de) 1995-04-27
CA2134042A1 (fr) 1995-04-27

Similar Documents

Publication Publication Date Title
DE2645614C3 (de) Verfahren zur Herstellung von Formkörpern aus einer härtenden Organopolysiloxanmasse
EP0455078B1 (fr) Elastomères silicone à déformation permanente sous pression réduite et procédé de leur préparation
EP0761723A2 (fr) Résine d'organopolysiloxanes liquides, procédé pour leur préparation, compositions de polydiorganosiloxanes à basse viscosité et leur application
DE69702370T2 (de) Härtbare Fluorosiloxanzusammensetzung und Verfahren zur Steuerung der Initiierung und der Dauer der Härtung
DE10259613A1 (de) Organopolysiloxanzusammensetzungen und deren Einsatz in bei Raumtemperatur vernetzbaren niedermoduligen Massen
EP0040750A1 (fr) Compositions d'organopolysiloxanes transformables en élastomères retardant la flamme
EP0587662B1 (fr) Melanges d'organo(poly)siloxanes pouvant etre reticules en elastomeres avec elimination d'alcools
DE10319303A1 (de) Verfahren zur Herstellung von vernetzbaren Massen auf der Basis von Organosiliciumverbindungen
EP0649877B1 (fr) Compositions autolubrifiantes
EP0010708B1 (fr) Procédé pour la préparation de masses d'organosiloxanes présentant une faible rémanence à la compression et qui sont durcissables en élastomères
EP1036820B1 (fr) Compositions organopolysiloxanes stables au stockage, réticulables en élastomères par élimination d'alcools
WO1999032551A1 (fr) Composes d'organopolysiloxane reticulables par clivage d'alcools pour donner des elastomeres
WO2002090431A1 (fr) Masses pouvant reticuler lors de la dissociation d'alcools composes de groupes terminaux alkoxysilyle en elastomeres
EP0057874A1 (fr) Compositions à mouler à base de polyorganosiloxanes
WO2002024813A1 (fr) Formulations de caoutchouc silicone et leur utilisation
EP2367868A1 (fr) Masses réticulables à base de composés organosilicium
EP1580214A1 (fr) Compositions réticulables à partir des composées organosilicones
DE69505197T2 (de) Feuchtigkeitshärtende Organosiloxan-Zusammensetzungen mit verlängerter Verarbeitungszeit
EP0852606B1 (fr) Masses d'organopolysiloxane reticulables en elastomeres avec separation d'alcools
EP1436351B1 (fr) Matieres reticulables a base de composes organosilicies
DE1795324C3 (de) Zu Elastomeren bei Zimmertemperatur unter Einwirkung von Wasser vulkanisierbare, in Abwesenheit desselben lagerfähige Organosiliciumformmassen
WO2021239222A1 (fr) Masses réticulables à base de composés d'organosilicium
DE1113567B (de) Verfahren zur Herstellung von fluorhaltigen Organopolysiloxan-elastomeren
EP1448695A1 (fr) Masses reticulables en elastomeres par separation d'alcools a partir de groupes alcoxysilyle terminaux
EP0218875A2 (fr) Composition de caoutchouc de siloxane durcissable

Legal Events

Date Code Title Description
PUAI Public reference made under article 153(3) epc to a published international application that has entered the european phase

Free format text: ORIGINAL CODE: 0009012

AK Designated contracting states

Kind code of ref document: A2

Designated state(s): AT BE CH DE ES FR GB IT LI NL SE

PUAL Search report despatched

Free format text: ORIGINAL CODE: 0009013

AK Designated contracting states

Kind code of ref document: A3

Designated state(s): AT BE CH DE ES FR GB IT LI NL SE

17P Request for examination filed

Effective date: 19960902

17Q First examination report despatched

Effective date: 19980629

RAP1 Party data changed (applicant data changed or rights of an application transferred)

Owner name: GE BAYER SILICONES GMBH & CO. KG

GRAG Despatch of communication of intention to grant

Free format text: ORIGINAL CODE: EPIDOS AGRA

GRAG Despatch of communication of intention to grant

Free format text: ORIGINAL CODE: EPIDOS AGRA

GRAH Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOS IGRA

GRAH Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOS IGRA

GRAA (expected) grant

Free format text: ORIGINAL CODE: 0009210

AK Designated contracting states

Kind code of ref document: B1

Designated state(s): AT BE CH DE ES FR GB IT LI NL SE

REF Corresponds to:

Ref document number: 200099

Country of ref document: AT

Date of ref document: 20010415

Kind code of ref document: T

REG Reference to a national code

Ref country code: CH

Ref legal event code: EP

REF Corresponds to:

Ref document number: 59409702

Country of ref document: DE

Date of ref document: 20010503

ITF It: translation for a ep patent filed
GBT Gb: translation of ep patent filed (gb section 77(6)(a)/1977)

Effective date: 20010529

ET Fr: translation filed
REG Reference to a national code

Ref country code: ES

Ref legal event code: FG2A

Ref document number: 2156887

Country of ref document: ES

Kind code of ref document: T3

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: AT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011013

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: SE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011014

Ref country code: ES

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011014

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: LI

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011031

Ref country code: CH

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011031

Ref country code: BE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20011031

REG Reference to a national code

Ref country code: GB

Ref legal event code: IF02

PLBE No opposition filed within time limit

Free format text: ORIGINAL CODE: 0009261

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: NO OPPOSITION FILED WITHIN TIME LIMIT

26N No opposition filed
BERE Be: lapsed

Owner name: GE BAYER SILICONES G.M.B.H. & CO. K.G.

Effective date: 20011031

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: NL

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20020501

EUG Se: european patent has lapsed

Ref document number: 94116179.6

REG Reference to a national code

Ref country code: CH

Ref legal event code: PL

NLV4 Nl: lapsed or anulled due to non-payment of the annual fee

Effective date: 20020501

REG Reference to a national code

Ref country code: ES

Ref legal event code: FD2A

Effective date: 20021113

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: IT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES;WARNING: LAPSES OF ITALIAN PATENTS WITH EFFECTIVE DATE BEFORE 2007 MAY HAVE OCCURRED AT ANY TIME BEFORE 2007. THE CORRECT EFFECTIVE DATE MAY BE DIFFERENT FROM THE ONE RECORDED.

Effective date: 20051013

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: GB

Payment date: 20131028

Year of fee payment: 20

Ref country code: DE

Payment date: 20131029

Year of fee payment: 20

Ref country code: FR

Payment date: 20131017

Year of fee payment: 20

REG Reference to a national code

Ref country code: DE

Ref legal event code: R071

Ref document number: 59409702

Country of ref document: DE

REG Reference to a national code

Ref country code: GB

Ref legal event code: PE20

Expiry date: 20141012

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: GB

Free format text: LAPSE BECAUSE OF EXPIRATION OF PROTECTION

Effective date: 20141012